The research field on perovskite solar cells (PSCs) is seeing frequent record breaking in the power conversion efficiency (PCE). However, organic-inorganic hybrid halide perovskites and organic additives in common hole-transport materials (HTMs) exhibit poor stability against moisture and heat. Here we report the successful fabrication of all-inorganic PSCs without any labile or expensive organic components. The entire fabrication process can be operated in ambient environment without humidity control (e.g., a glovebox). Even without encapsulation, the all-inorganic PSCs present no performance degradation in humid air (90-95% relative humidity, 25 °C) for over 3 months (2640 h) and can endure extreme temperatures (100 and -22 °C). Moreover, by elimination of expensive HTMs and noble-metal electrodes, the cost was significantly reduced. The highest PCE of the first-generation all-inorganic PSCs reached 6.7%. This study opens the door for next-generation PSCs with long-term stability under harsh conditions, making practical application of PSCs a real possibility.

The emergence of perovskite solar cells (PSCs) has generated enormous interest in the photovoltaic research community. Recently, cesium metal halides (CsMX, M = Pb or Sn; X = I, Br, Cl or mixed halides) as a class of inorganic perovskites showed great promise for PSCs and other optoelectronic devices. However, CsMX-based PSCs usually exhibit lower power conversion efficiencies (PCEs) than organic-inorganic hybrid PSCs, due to the unfavorable band gaps. Herein, a novel mixed-Pb/Sn mixed-halide inorganic perovskite, CsPbSnIBr, with a suitable band gap of 1.79 eV and an appropriate level of valence band maximum, was prepared in ambient atmosphere without a glovebox. After thoroughly eliminating labile organic components and noble metals, the all-inorganic PSCs based on CsPbSnIBr and carbon counter electrodes exhibit a high open-circuit voltage of 1.26 V and a remarkable PCE up to 11.33%, which is record-breaking among the existing CsMX-based PSCs. Moreover, the all-inorganic PSCs show good long-term stability and improved endurance against heat and moisture. This study indicates a feasible way to design inorganic halide perovskites through energy-band engineering for the construction of high-performance all-inorganic PSCs.

In this work all‐inorganic perovskite CsPbIBr2 are doped with Mn to compensate their shortcomings in band structure for the application of perovskite solar cells (PSCs). The novel Mn‐doped all‐inorganic perovskites, CsPb1−xMnxI1+2xBr2−2x, are prepared in ambient atmosphere. As the concentration of Mn2+ ions increases, the bandgaps of CsPb1−xMnxI1+2xBr2−2x decrease from 1.89 to 1.75 eV. Additionally, when the concentration of Mn dopants is appropriate, this novel Mn‐doped all‐inorganic perovskite film shows better crystallinity and morphology than its undoped counterpart. These advantages alleviate the energy loss in hole transfer and facilitate the charge‐transfer in perovskites, therefore, PSCs based on these novel CsPb1−xMnxI1+2xBr2−2x perovskite films display better photovoltaic performance than the undoped CsPbIBr2 perovskite films. The reference CsPbIBr2 cell reaches a power conversion efficiency (PCE) of 6.14%, comparable with the previous reports. The CsPb1−xMnxI1+2xBr2−2x cells reach the highest PCE of 7.36% (when x = 0.005), an increase of 19.9% in PCE. Furthermore, the encapsulated CsPb0.995Mn0.005I1.01Br1.99 cells exhibit good stability in ambient atmosphere. The storage stability measurements on the encapsulated PSCs reveal that PCE is dropped by only 8% of the initial value after >300 h in ambient. Such improved efficiency and stability are achieved using low‐cost carbon electrodes (without expensive hole transport materials and Au electrodes).

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